University of Dundee

100 years of suramin Wiedemar, Natalie; Hauser, Dennis A.; Mäser, Pascal

Published in: Antimicrobial Agents and Chemotherapy

DOI: 10.1128/AAC.01168-19

Publication date: 2020

Document Version Peer reviewed version

Link to publication in Discovery Research Portal

Citation for published version (APA): Wiedemar, N., Hauser, D. A., & Mäser, P. (2020). 100 years of suramin. Antimicrobial Agents and Chemotherapy, 64(3), 1-14. [e01168]. https://doi.org/10.1128/AAC.01168-19

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1 One Hundred Years of Suramin http://aac.asm.org/ 2 3 4 Natalie Wiedemar1,2, Dennis A. Hauser1,2 and Pascal Mäser1,2 5 6 7 1 Swiss Tropical and Public Health Institute on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 8 Dept. Medical Parasitology and Infection Biology 9 Socinstrasse 57 10 4051 Basel 11 Switzerland 12 13 2 University of Basel 14 Petersplatz 1 15 4001 Basel 16 Switzerland Downloaded from

17 Abstract http://aac.asm.org/ 18 Suramin is a hundred years old and still being used to treat the first stage of acute human sleeping

19 sickness, caused by brucei rhodesiense. Suramin is a multifunctional with a

20 wide array of potential applications, from parasitic and viral diseases to cancer, snakebite and

21 . Suramin is also an enigmatic molecule: What are its targets? And how does it get into cells

22 in the first place? Here we provide an overview on the many different candidate targets of suramin, on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

23 discuss modes of action, and routes of cellular uptake. We reason that once the polypharmacology

24 of suramin is understood at the molecular level, new, more specific, and less toxic can be

25 identified for the numerous potential applications of suramin.

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26 Suramin, the fruit of early medicinal chemistry http://aac.asm.org/ 27 When suramin was introduced for the treatment of African sleeping sickness in 1922, it was one of

28 the first anti-infective agents that had been developed in a medicinal chemistry program. Starting

29 from the antitrypanosomal activity of the dye , synthesized in 1904 by Paul Ehrlich,

30 made a series of colorless and more potent derivatives. Molecule 205 was suramin (Figure 1),

31 synthesized by Oskar Dressel, Richard Kothe and Bernhard Heymann in 1916. Sleeping sickness on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

32 (also known as human African , HAT) was at the forefront of research at that time,

33 not a neglected disease as it is today, and the development of suramin was a breakthrough for the

34 emerging field of chemotherapy. While the history of suramin has been reviewed elsewhere (1), we

35 focus here on the many potential applications of suramin and its enigmatic mode of action.

36

37 Suramin as an drug

38 Suramin is still being used for the treatment of rhodesiense infections (2).

39 However, it does not cross the blood-brain barrier and therefore is administered only for the first,

40 hemolymphatic stage of sleeping sickness, when the trypanosomes have not yet invaded the

41 patient's CNS. The standard treatment regimen for suramin is an initial test dose of 4-5 mg/kg

42 followed by five weekly doses of 20 mg/kg (but not more than 1 g) injected i.v. (3). Suramin is also

43 used for Surra (mal de caderas), caused by T. evansi, in particular for the treatment of camels (4).

44 The treatment regimen is a single injection i.v. of 10 mg/kg suramin, i.e. about 6-10 g (4). In vitro,

45 suramin also has some activity against T. cruzi (5). However, it is not used for Chagas' disease, and

46 studies in mice even suggested that suramin would exacerbate the disease (6). In vitro activity of

47 suramin against Leishmania major and L. donovani has recently been described (7). Furthermore,

48 suramin blocks host cell invasion by the malaria parasite Plasmodium falciparum. This was

49 observed for both the invasion of erythrocytes by P. falciparum merozoites (8) and the invasion of

50 HepG2 hepatoma cells by P. falciparum sporozoites (9).

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51 Suramin had been in use for river blindness, caused by the filarial parasite Onchocerca http://aac.asm.org/ 52 volvulus (10). It acts on both microfilariae and, to a larger extent, on adult worms (11, 12).

53 However, suramin was subsequently replaced by the less toxic, and orally bioavailable,

54 (13, 14). The adverse effects of suramin are indeed manifold, including nephrotoxicity,

55 hypersensitivity reactions, dermatitis, anemia, peripheral neuropathy and bone marrow toxicity (3,

56 15). But despite its potential toxicity, the lack of bioavailability, and absence of lead-like properties on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

57 (Figure 1), suramin has found a surprising variety of repurposing applications. Table 1 provides an

58 overview on the biological activities of suramin and Table 2 lists clinical trials performed with

59 suramin.

60

61 Suramin as an antiviral agent

62 The antiviral and antibacteriophage activities of suramin are known since the mid-20th century (19,

63 20). Soon after the discovery of retroviruses, suramin was found to inhibit retroviral reverse

64 transcriptase (21), which served as a rationale to test suramin against human immunodeficiency

65 virus (HIV). Suramin protected T-cells from HIV infection in vitro (22), and in AIDS patients it

66 reduced the viral burden in some of the study subjects; however, no improvement of the

67 immunological features and clinical symptoms was achieved (17, 23, 24). Later-on suramin was

68 found to inhibit host cell attachment through binding to the HIV-1 envelope glycoprotein gp120,

69 indicating that the in vitro protection against HIV infection is mediated through inhibition of viral

70 entry (25).

71 Suramin also inhibits the binding of Dengue virus to host cells through a direct effect on the

72 viral envelope protein (26). Inhibition of host cell attachment was also found for Herpes

73 simplex (27) and Hepatitis C viruses (28), which explained the previously reported protective

74 effects of suramin against in vitro herpes simplex infections (29) and in vivo infections of ducks

75 with Duck Hepatitis B Virus (30). Similar to the experience with HIV, suramin had initially been

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76 tested against Hepatitis viruses due to its inhibitory effect on the viral DNA polymerase (31, 32). http://aac.asm.org/ 77 But in a small suramin was found to be ineffective and toxic in chronic active Hepatitis

78 B patients (18). Suramin neutralized enterovirus 71 (EV71) in cell culture and in a mouse model by

79 binding to capsid proteins (33–35).

80 Suramin also bears potential against emerging viruses. It was shown to inhibit both RNA

81 synthesis and replication in Chikungunya virus (36). In vitro suramin conferred protection if present on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

82 at the time of infection, and this was attributed to a reduction of viral host cell binding and

83 uptake (37). In the murine model suramin led to a reduction of pathognomonic lesions if injected

84 prior to Chikungunya infection (38). Suramin also inhibited host cell invasion by Ebola virus (39)

85 and Zika virus, even when added after viral exposure of the cell cultures (40).

86

87 Suramin against cancer

88 The first studies on the effects of suramin on neoplasms in animals were carried out in the 1940's;

89 mice engrafted with lymphosarcoma developed significantly smaller tumors when simultaneously

90 treated with suramin (41). In the 1970's it was shown that suramin can enhance the action of

91 and adriamycin in mice engrafted with Ehrlich carcinoma (42). A first clinical

92 trial with suramin was carried out in the 1980's in advanced-stage adrenal and renal cancer

93 patients (16). Around half of the patients showed either partial or minimal responses, none showed

94 complete remission. Nevertheless, a number of subsequent clinical trials with suramin were carried

95 out (Table 2). In particular, suramin was tested against (43–51), non-small cell lung

96 cancer (52), breast cancer (52), bladder cancer (53, 54) and brain tumors (55, 56). Most of these

97 studies were based on the potential of suramin to act as an antagonist of growth factors (57–59),

98 which are often overexpressed by tumors. In addition, suramin directly exhibits cytostatic activity

99 on cultured tumor cells (60–62). However, the initial clinical tests did not warrant the further

100 development of suramin as an anticancer monotherapy.

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101 Subsequent tests focused on suramin as a chemosensitizer, based on the findings that at sub- http://aac.asm.org/ 102 cytotoxic levels (<50 µM), it enhanced the efficacy of anticancer drugs such as mitomycin C, taxol

103 or doxorubicin in ex vivo cultures and in animal models (63–65). Suramin combined with taxol

104 inhibited invasiveness and prevented metastasis in a xenograft mouse model (66). Different

105 explanations are conceivable for the chemosensitizing effects of suramin on tumor cells, including

106 inhibition of telomerase (67) or inhibition of fibroblast growth factors and angiogenesis (68). A on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

107 phase II clinical study was performed in patients with advanced, drug-resistant, non-small cell lung

108 cancer treated with taxol or carboplatin; supplementation with nontoxic doses of suramin did not

109 overcome drug resistance (69). Randomized controlled studies to validate the use of suramin as a

110 chemosensitizer in chemotherapy-naive lung cancer patients remain to be performed. A

111 combination of estramustine, and suramin gave promising results in hormone-refractory

112 prostate cancer patients (51).

113

114 Suramin as an antidote

115 Three of the many biological activities of suramin support a potential use as a protective agent: the

116 inhibition of thrombin, the inhibition of phospholipase A2, and the inhibition of purinergic

117 signaling. Several vipers possess toxins that mimic thrombin (70), perfidiously triggering the

118 coagulation cascade in the mammalian blood. Suramin not only inhibits thrombin itself (71) but

119 also the thrombin-like proteases of snake venom (72), and was therefore proposed as an antidote for

120 snakebite. Other common constituents of metazoan venoms are phospholipases A2 that convert

121 phospholipids into lysophospholipids. Again, suramin inhibits mammalian phospholipase A2 (73)

122 as well as the orthologs from snake venom (74–76) and bee venom (77), suggesting that it can act

123 as an antidote. A certain degree of protection from venoms by suramin was confirmed in mouse

124 models (77–79). The potential use of suramin as an antidote is attractive given the high global

125 burden of snakebites (80) and the current shortage of antivenom (81).

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126 Suramin's ability to block P2 purinergic, G protein-coupled receptors (82) may counteract http://aac.asm.org/ 127 the action of neurotoxins that trigger arachidonic acid signaling, e.g. via phospholipase A2

128 activity (83). A possible explanation is that suramin prevents the activation of ATP receptors at the

129 motor nerve ending, which otherwise would depress Ca2+ currents and reduce acetylcholine release

130 at the presynaptic membrane (84). Suramin was also proposed to serve as a neuroprotective

131 agent (85, 86), as an antidote for kidney toxicity during cancer chemotherapy (87) and, based on its on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

132 antiapoptotic effect, to protect from liver failure (88). Suramin also inhibits connexin channels of

133 the tight junction, thereby suppressing ATP release and protecting cells from pore-forming bacterial

134 toxins such as hemolysin (89). The suramin analogs NF340 and NF546 were cardioprotective in a

135 mouse model for heart graft rejection, presumably via inhibition of the purinergic G protein-coupled

136 P2Y11 (90).

137

138 Further potential uses of suramin

139 Suramin was found to have beneficial effects in a rat arthritis model (91) and to suppress fear

140 responses in the rat (92). It also promoted the expansion of T cells during immunization of mice and

141 was therefore considered as a small molecule adjuvant for vaccination (93). Based on the cell

142 danger hypothesis, suramin has recently been tested for the treatment of autism spectrum disorders

143 (ASD). The cell danger hypothesis suggests that a systemic stress response, which involves

144 mitochondria and purinergic signaling, contributes to the development of psychopathologies like

145 autism. Suramin had been shown to act as an inhibitor of purinergic signaling (94) and

146 mitochondrial function (95), and was therefore proposed as a potential therapy for ASD (96). First

147 tests in mouse models showed correction of symptoms in juveniles (96) as well as in adults (97). A

148 first small human trial was carried out and, even though difficult to quantify, showed improvement

149 of ASD symptoms (98).

150

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151 (Too) many targets http://aac.asm.org/ 152 Suramin is a large molecule that carries six negative charges at physiological pH (Figure 1). It is

153 likely to bind to, and thereby inhibit, various proteins (99). Thus the many and diverse potential

154 applications of suramin reflect the polypharmacology of suramin. Indeed, a large number of

155 have been shown to be inhibited by suramin (Table 3). Suramin inhibits many glycolytic

156 enzymes (100, 101), enzymes involved in galactose catabolism (PubChem BioAssay: 493189) and on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

157 enzymes of the Krebs cycle (102). Suramin further decreases the activity of a large number of

158 enzymes involved in DNA and RNA synthesis and modification: DNA polymerases (103, 104),

159 RNA polymerases (103, 105, 106), reverse transcriptase (21, 103), telomerase (67), and enzymes

160 involved in winding/unwinding of DNA (107, 108) are inhibited by suramin, as well as histone- and

161 chromatin modifying enzymes like chromobox proteins (109), methyltransferases (110) and sirtuin

162 histone deacetylases (111). Suramin is also an inhibitor of other sirtuins (112) and protein kinases

163 (113, 114), glutaminase (PubChem BioAssay: 624170), phospholipase A2 (115, 116), protein

164 tyrosine phosphatases (117), lysozyme (118) and different serine- and cysteine-proteases (119–

165 121). For caspases, cysteine proteases involved in apoptosis, suramin was described to act as either

166 inhibitor or activator (122, 123). Suramin further inhibits the Na+,K+-ATPase and other ATPases

167 (124–126), certain classes of GABA receptors (127, 128), and several G protein-coupled

168 receptors (129) including P2 purinoceptors and follicle-stimulating hormone receptor (130, 131).

169 Suramin also showed inhibitory effects against components of the coagulation cascade (71, 132)

170 and the complement system (133–135), and against deubiquitinating enzymes (PubChem BioAssay:

171 504865; 463106). It also interacts with prion protein, inhibiting the conversion into the pathogenic

172 form PrPSc (136). Beside the many inhibitory activities, suramin also activates certain nuclear

173 receptors that act as transcription factors (137), and intracellular channels (138).

174

175

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176 Enigmatic mechanisms of action against African trypanosomes http://aac.asm.org/ 177 Somewhat ironically, much less appears to be known about the targets of suramin in African

178 trypanosomes, where it has been in use for a century, than in tumor cells or viruses. Suramin was

179 shown to inhibit glycolytic enzymes of T. brucei with selectivity over their mammalian orthologues,

180 in particular hexokinase, aldolase, phosphoglycerate kinase and glycerol-3-phosphate

181 dehydrogenase (100). Intriguingly, the trypanosomal enzymes have higher isoelectric points (>9), on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

182 which is due to extra arginines and lysines that are absent in the mammalian orthologues (165).

183 These residues form positively charged, surface exposed 'hot spots' that were proposed to be bound

184 by the negatively charged suramin (100). Inhibition of trypanosomal by suramin is in

185 agreement with the dose-dependent inhibition of oxygen consumption and ATP production

186 observed in trypanosomes isolated from suramin-treated rats (166). However, the glycolytic

187 enzymes of T. brucei are localized inside glycosomes (167), and it is unclear how suramin could

188 penetrate the glycosomal membrane, or if suramin could bind to glycolytic enzymes in the cytosol,

189 before they are imported into the glycosomes (168). Alternative targets proposed for the

190 trypanocidal effect of suramin are glycerophosphate oxidase (139, 169), a serine oligopeptidase

191 termed OP-Tb (170), and REL1 (171), the RNA-editing ligase of the trypanosome's kinetoplast. It is

192 unclear how suramin would pass the inner mitochondrial membrane, but suramin inhibited

193 oxidative phosphorylation in mitochondrial preparations of the trypanosomatid Crithidia

194 fasciculate (172). Suramin also appeared to inhibit cytokinesis in T. brucei, as indicated by the

195 finding that suramin treatment resulted in an increased number of trypanosomes with two

196 nuclei (173).

197

198 Uptake routes of suramin into cells

199 The negative charges of suramin (Figure 1) not only promote binding to various proteins, they also

200 prevent diffusion across biological membranes. However, the majority of targets (Table 3) are

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201 intracellular, and radiolabeled suramin was shown to be taken up by human endothelial and http://aac.asm.org/ 202 carcinoma cells (174, 175) and by T. brucei bloodstream forms (166, 176). Suramin is not a

203 substrate of P-glycoprotein (177), nor of any other known transporter. Thus suramin must be

204 imported by endocytosis. Mammalian cells can take up suramin in complex with serum albumin by

205 receptor-mediated endocytosis (178). This had originally also been thought to happen in T.

206 brucei (166). However, the trypanosomes do not take up albumin by receptor-mediated on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

207 endocytosis (179), and LDL (low density lipoprotein) was proposed to act as the vehicle

208 instead (176). Suramin bound to LDL and inhibited the binding and uptake of LDL, while LDL

209 enhanced the uptake of suramin in bloodstream-form T. brucei (176). In contrast, overexpression in

210 procyclic T. b. brucei of Rab4, a small GTPase involved in the recycling of endosomes, decreased

211 suramin binding and uptake without affecting LDL binding or uptake (180). In the same study,

212 overexpression of a mutant Rab5, which was locked in the active, GTP-bound form, increased LDL

213 uptake without affecting suramin uptake (180). These findings indicated that, at least in the

214 procyclic trypanosomes of the tsetse fly midgut, LDL and suramin are imported independently of

215 each other.

216 The development of genome-wide RNAi screens in bloodstream-form T. brucei combined

217 with next-generation sequencing offered new opportunities to address the genetics of drug

218 resistance. This approach identified genes, silencing of which reduced the sensitivity to

219 suramin (181). These included a number of genes encoding for endosomal and lysosomal proteins,

220 in agreement with uptake of suramin through endocytosis. The invariant surface glycoprotein

221 ISG75 was identified as a likely receptor of suramin since knock-down of ISG75 in bloodstream-

222 form T. brucei decreased suramin binding and suramin susceptibility (181). ISG75 is a surface

223 protein of unknown function whose abundance is controlled by ubiquitination (182). Thus, there

224 appear to be (at least) two pathways for receptor-mediated endocytosis of suramin in T. brucei

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225 bloodstream forms: either directly with ISG75 as the receptor or, after binding of suramin to LDL, http://aac.asm.org/ 226 together with the LDL receptor.

227

228 Conclusion

229 Suramin remains controversial. Is its polypharmacology a liability or an asset? Is it toxic or

230 protective? Dated or timeless? Whatever the verdict on suramin, there is hardly a molecule with as on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

231 many biological activities. The list of potential targets is indeed impressive, and the publication

232 stream on suramin is not stagnating. The large majority of papers is not about trypanosomes or

233 trypanosomiasis (Figure 2). The list of potential targets has to be taken with a grain of salt, though,

234 since the negative charges of suramin, and its promiscuity in protein binding, can cause all kinds of

235 artefacts. Suramin can dissolve matrigel (183), resulting in a false positive signal in cell-based

236 screening campaigns that use matrigel for support, e.g. for inhibitors of angiogenesis (183). On the

237 other hand, suramin's high affinity to albumin (184) may give false negative results in cell-based

238 tests that contain mammalian serum. But in spite of the various confounders, a number of different

239 drug-target interactions for suramin have been experimentally validated, and are directly supported

240 by crystal structures (Table 4).

241 Several routes of investigation on the bioactivities of suramin have culminated in clinical

242 trials with healthy volunteers (i.e. phase I) or patients (i.e. phases II and III; Table 2). Yet, to our

243 knowledge, none of these trials was a striking success, and it is unclear whether suramin will ever

244 find medical applications outside the field of parasitology. However, molecules that act in a similar

245 way than suramin may be identified via target-based screening once the mode of action is

246 understood – new molecules that are more specific, less toxic, and possess better pharmacological

247 properties than suramin. Thus it will be important to dissect the polypharmacology of suramin at the

248 molecular level. We hope that the compiled list of targets (Table 3) will serve this purpose.

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249 Acknowledgments http://aac.asm.org/ 250 We are grateful to the Swiss National Science Foundation for financial support and to Prof. Alan

251 Fairlamb for sharing insights into the possible molecular interactions of suramin. on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

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662 CP, Xia M. 2011. Identification of clinically used drugs that activate pregnane X on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 663 receptors. Drug Metab Dispos Biol Fate Chem 39:151–159.

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665 Hohenegger M. 1999. Suramin and suramin analogs activate skeletal muscle

666 via a calmodulin binding site. Mol Pharmacol 55:462–472.

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668 trypanocidal compounds’ effects on sn-glycerol-3-phosphate oxidase. Exp Parasitol

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670 140. Dias DA, de Barros Penteado B, Dos Santos LD, Dos Santos PM, Arruda CCP,

671 Schetinger MRC, Leal DBR, Dos Santos Jaques JA. 2017. Characterization of

672 ectonucleoside triphosphate diphosphohydrolase (E-NTPDase; EC 3.6.1.5) activity

673 in mouse peritoneal cavity cells. Cell Biochem Funct 35:358–363.

674 141. Oses JP, Cardoso CM, Germano RA, Kirst IB, Rücker B, Fürstenau CR, Wink MR,

675 Bonan CD, Battastini AMO, Sarkis JJF. 2004. Soluble NTPDase: An additional

676 system of hydrolysis in rat blood serum. Life Sci 74:3275–3284.

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678 Silva E Bastos M, Castro FF de, Oliveira CM de, Borges-Pereira L, de Souza ACA,

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691 activity of HIV-1 reverse transcriptase: further biochemical characterization and

692 search of inhibitors. Biochimie 75:127–134.

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695 2012. Identification and analysis of hepatitis C virus NS3 helicase inhibitors using

696 nucleic acid binding assays. Nucleic Acids Res 40:8607–8621.

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703 HuR functions and attenuates malignant phenotype of oral cancer cells. Cancer

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707 The anti-parasitic agent suramin and several of its analogues are inhibitors of the

708 DNA binding protein Mcm10. Open Biol 9:190117.

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710 H. 2013. Assay development for histone methyltransferases. Assay Drug Dev

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713 Coronado MA. 2019. Binding studies of a putative C. pseudotuberculosis target

714 protein from Vitamin B12 Metabolism. Sci Rep 9:6350.

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716 Chung P, Kisielewski A, Zhang L-L, Scherer B, Sinclair DA. 2003. Small molecule

717 activators of sirtuins extend Saccharomyces cerevisiae lifespan. Nature 425:191–

718 196.

719 153. Trueblood KE, Mohr S, Dubyak GR. 2011. Purinergic regulation of high-glucose-

720 induced caspase-1 activation in the rat retinal Müller cell line rMC-1. Am J Physiol

721 Cell Physiol 301:C1213-1223.

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725 13:197–207.

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728 156. Beiler JM, Martin GJ. 1948. Inhibition of hyaluronidase action by derivatives of

729 hesperidin. J Biol Chem 174:31–35.

730 157. Constantopoulos G, Rees S, Cragg BG, Barranger JA, Brady RO. 1980.

731 Experimental animal model for mucopolysaccharidosis: suramin-induced

732 glycosaminoglycan and sphingolipid accumulation in the rat. Proc Natl Acad Sci U S

733 A 77:3700–3704.

734 158. Bachmann A, Russ U, Quast U. 1999. Potent inhibition of the CFTR chloride

735 channel by suramin. Naunyn Schmiedebergs Arch Pharmacol 360:473–476.

736 159. Peoples RW, Li C. 1998. Inhibition of NMDA-gated ion channels by the P2

737 purinoceptor antagonists suramin and reactive blue 2 in mouse hippocampal

738 neurones. Br J Pharmacol 124:400–408.

739 160. Sharma A, Yogavel M, Sharma A. 2016. Structural and functional attributes of

740 malaria parasite diadenosine tetraphosphate hydrolase. Sci Rep 6:19981.

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744 162. Quemé-Peña M, Juhász T, Mihály J, Cs Szigyártó I, Horváti K, Bősze S, Henczkó J,

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747 Polysulfonated Drug Suramin: A Step Closer to in Vivo Complexity. Chembiochem

748 Eur J Chem Biol.

749 163. Abdeen S, Salim N, Mammadova N, Summers CM, Goldsmith-Pestana K,

750 McMahon-Pratt D, Schultz PG, Horwich AL, Chapman E, Johnson SM. 2016.

751 Targeting the HSP60/10 chaperonin systems of Trypanosoma brucei as a strategy

752 for treating African sleeping sickness. Bioorg Med Chem Lett 26:5247–5253.

753 164. Stevens M, Abdeen S, Salim N, Ray A-M, Washburn A, Chitre S, Sivinski J, Park Y,

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755 inhibited by a variety of approved drugs, natural products, and known bioactive

756 molecules. Bioorg Med Chem Lett 29:1106–1112.

757 165. Wierenga RK, Swinkels B, Michels PA, Osinga K, Misset O, Van Beeumen J,

758 Gibson WC, Postma JP, Borst P, Opperdoes FR. 1987. Common elements on the

759 surface of glycolytic enzymes from Trypanosoma brucei may serve as topogenic

760 signals for import into glycosomes. EMBO J 6:215–221.

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763 rate in vivo. Mol Biochem Parasitol 1:315–333.

764 167. Opperdoes FR, Borst P. 1977. Localization of nine glycolytic enzymes in a

765 microbody-like organelle in Trypanosoma brucei: the glycosome. FEBS Lett 80:360– on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 766 364.

767 168. Wang CC. 1995. Molecular mechanisms and therapeutic approaches to the

768 treatment of African trypanosomiasis. Annu Rev Pharmacol Toxicol 35:93–127.

769 169. Fairlamb A. 1975. A study of glycerophosphate oxidase in Trypanosoma brucei.

770 Ph.D. Thesis, University of Edinburgh.

771 170. Morty RE, Troeberg L, Pike RN, Jones R, Nickel P, Lonsdale-Eccles JD, Coetzer

772 TH. 1998. A trypanosome oligopeptidase as a target for the trypanocidal agents

773 , diminazene and suramin. FEBS Lett 433:251–256.

774 171. Zimmermann S, Hall L, Riley S, Sørensen J, Amaro RE, Schnaufer A. 2016. A novel

775 high-throughput activity assay for the Trypanosoma brucei editosome enzyme REL1

776 and other RNA ligases. Nucleic Acids Res 44:e24.

777 172. Roveri OA, Franke de Cazzulo BM, Cazzulo JJ. 1982. Inhibition by suramin of

778 oxidative phosphorylation in Crithidia fasciculata. Comp Biochem Physiol B 71:611–

779 616.

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780 173. Thomas JA, Baker N, Hutchinson S, Dominicus C, Trenaman A, Glover L, Alsford S, http://aac.asm.org/ 781 Horn D. 2018. Insights into antitrypanosomal drug mode-of-action from cytology-

782 based profiling. PLoS Negl Trop Dis 12:e0006980.

783 174. Gagliardi AR, Taylor MF, Collins DC. 1998. Uptake of suramin by human

784 microvascular endothelial cells. Cancer Lett 125:97–102. on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

785 175. Baghdiguian S, Boudier JL, Boudier JA, Fantini J. 1996. Intracellular localisation of

786 suramin, an anticancer drug, in human colon adenocarcinoma cells: a study by

787 quantitative autoradiography. Eur J Cancer Oxf Engl 1990 32A:525–532.

788 176. Vansterkenburg EL, Coppens I, Wilting J, Bos OJ, Fischer MJ, Janssen LH,

789 Opperdoes FR. 1993. The uptake of the trypanocidal drug suramin in combination

790 with low-density lipoproteins by Trypanosoma brucei and its possible mode of

791 action. Acta Trop 54:237–250.

792 177. Sanderson L, Khan A, Thomas S. 2007. Distribution of suramin, an

793 antitrypanosomal drug, across the blood-brain and blood-cerebrospinal fluid

794 interfaces in wild-type and P-glycoprotein transporter-deficient mice. Antimicrob

795 Agents Chemother 51:3136–3146.

796 178. Baghdiguian S, Boudier JL, Boudier JA, Fantini J. 1996. Intracellular localisation of

797 suramin, an anticancer drug, in human colon adenocarcinoma cells: a study by

798 quantitative autoradiography. Eur J Cancer Oxf Engl 1990 32A:525–532.

799 179. Coppens I, Opperdoes FR, Courtoy PJ, Baudhuin P. 1987. Receptor-mediated

800 endocytosis in the bloodstream form of Trypanosoma brucei. J Protozool 34:465–

801 473.

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802 180. Pal A, Hall BS, Field MC. 2002. Evidence for a non-LDL-mediated entry route for the http://aac.asm.org/ 803 trypanocidal drug suramin in Trypanosoma brucei. Mol Biochem Parasitol 122:217–

804 221.

805 181. Alsford S, Eckert S, Baker N, Glover L, Sanchez-Flores A, Leung KF, Turner DJ,

806 Field MC, Berriman M, Horn D. 2012. High-throughput decoding of antitrypanosomal on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 807 drug efficacy and resistance. Nature 482:232–236.

808 182. Zoltner M, Leung KF, Alsford S, Horn D, Field MC. 2015. Modulation of the Surface

809 Proteome through Multiple Ubiquitylation Pathways in African Trypanosomes. PLoS

810 Pathog 11:e1005236.

811 183. Prigozhina NL, Heisel AJ, Seldeen JR, Cosford NDP, Price JH. 2013. Amphiphilic

812 suramin dissolves Matrigel, causing an “inhibition” artefact within in vitro

813 angiogenesis assays. Int J Exp Pathol 94:412–417.

814 184. Vansterkenburg EL, Wilting J, Janssen LH. 1989. Influence of pH on the binding of

815 suramin to human serum albumin. Biochem Pharmacol 38:3029–3035.

816 185. Lozano RM, Jiménez M, Santoro J, Rico M, Giménez-Gallego G. 1998. Solution

817 structure of acidic fibroblast growth factor bound to 1,3, 6-naphthalenetrisulfonate: a

818 minimal model for the anti-tumoral action of suramins and suradistas. J Mol Biol

819 281:899–915.

820 186. Huang H-W, Mohan SK, Yu C. 2010. The NMR solution structure of human

821 epidermal growth factor (hEGF) at physiological pH and its interactions with

822 suramin. Biochem Biophys Res Commun 402:705–710.

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823 187. Lima LMTR, Becker CF, Giesel GM, Marques AF, Cargnelutti MT, de Oliveira Neto http://aac.asm.org/ 824 M, Monteiro RQ, Verli H, Polikarpov I. 2009. Structural and thermodynamic analysis

825 of thrombin:suramin interaction in solution and crystal phases. Biochim Biophys

826 Acta 1794:873–881.

827 188. Jiao L, Ouyang S, Liang M, Niu F, Shaw N, Wu W, Ding W, Jin C, Peng Y, Zhu Y, on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 828 Zhang F, Wang T, Li C, Zuo X, Luan C-H, Li D, Liu Z-J. 2013. Structure of severe

829 with thrombocytopenia syndrome virus nucleocapsid protein in complex with

830 suramin reveals therapeutic potential. J Virol 87:6829–6839.

831

832

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833 TABLES http://aac.asm.org/ 834

835 Table 1. Diseases and pathogens susceptible to suramin.

836

Activity in Activity in Activity in Disease, pathogen cell culture animal model patient on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

Parasitic infections T. b. rhodesiense HAT x x x T. b. gambiense HAT x x x Surra, T. evansi x x n.a. River blindness, O. volvulus x x x Trypanosoma cruzi x Leishmania spp. x Plasmodium falciparum x Viral infections Hepatitis x x x AIDS, HIV x x Herpes simplex x x Chikungunya x x Enterovirus 71 x x Dengue x Zika x Ebola x Neoplastic diseases Non-small cell lung cancer x x Breast cancer x x Bladder cancer x x Brain tumors x x Prostate cancer x x x Other uses Snake bite x x Arthritis x x Autism n.a. x x 837

838

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839 Table 2. Clinical trials with suramin. Trials with a registered NCT number are from http://aac.asm.org/ 840 ClinicalTrials.gov; others are from the literature.

841

Registry ID Disease Phase Year

NCT02508259 Autism spectrum disorders I, II 2015

NCT01671332 Non-small cell lung cancer II 2012 on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre NCT01038752 Non-small cell lung cancer II 2010 NCT00083109 Recurrent renal cell carcinoma I, II 2004 NCT00066768 Recurrent non-small cell lung cancer I 2003 NCT00054028 Recurrent breast cancer I, II 2002 NCT00006929 Recurrent non-small cell lung cancer II 2000 NCT00006476 Bladder cancer I 2000 NCT00004073 Brain and central nervous system tumors II 1999 NCT00002921 Adrenocortical carcinoma II 1997 NCT00003038 Advanced solid tumors I 1997 NCT00002723 Prostate cancer III 1996 NCT00002881 Prostate cancer III 1996 NCT00002652 Multiple myeloma and plasma cell neoplasm II 1995 NCT00002639 Brain and central nervous system tumors II 1995 NCT00001381 Bladder neoplasms, transitional cell carcinoma I 1994 NCT00001266 Prostatic neoplasm II 1990 NCT00001230 Filariasis observ. 1988 (16) Solid tumors observ. 1987 (17) AIDS observ. 1987 (18) Hepatitis B observ. 1987 842

843

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844 Table 3. Putative target proteins of suramin, biological processes and mechanisms. Suramin acts as http://aac.asm.org/ 845 an inhibitor or antagonist in all cases except for the and the ryanodine receptor.

846 The mode of action against caspase is controversial.

847

Putative target Reference

on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre Metabolism 6-Phosphofructokinase (100) Fructose-l,6-bisphosphate aldolase (100) Glucose-6-phosphate isomerase (100) Glyceraldehyde-3-phosphate dehydrogenase (100) Glycerol-3-phosphate dehydrogenase (100, 139) Glycerol kinase (100) Hexokinase (100) Phosphoglycerate kinase (100) Pyruvate kinase (101) Triose-phosphate isomerase (100) Succinic dehydrogenase (102) Galactokinase 493189* Glutaminase 624170* Glycerophosphate oxidase (139) Nucleoside triphosphate diphosphohydrolase 1 & 2 (125, 126, 140–143) Nucleotide pyrophosphatase/phosphodiesterase 1 & 3 (144)

Nucleic acids DNA polymerase alpha (103, 104) DNA polymerase beta (103, 104) DNA polymerase gamma (103) DNA polymerase delta (104) DNA polymerase I (103, 104) Terminal deoxynucleotidyltransferase (103) DNA primase (103) DNA dependent RNA polymerase (103, 106) RNA dependent RNA polymerase (105) Reverse transcriptase (21, 103) Telomerase (67) RNAse H (145) Flavivirus RNA helicase (40, 107, 146) DNA Topoisomerase II (108) Tyrosyl-DNA phosphodiesterase 1 (147) Human antigen R (148) DNA-binding protein MCM10 (149)

Epigenetics Chromobox protein homologue 1 beta 488953* Chromobox protein homologue 7 (109) Histone methyltransferases (110, 150) Precorrin-4 C(11)-methyltransferase (151) Sirtuin 1, 2, 5 (111, 112, 152)

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Protease http://aac.asm.org/ Kallikrein (121) Alpha Thrombin (71) Human neutrohphil cathepsing G (120) Human neutrophil elastase (120) Human neutrophil proteinase 3 (120) Rhodesain (119) Caspases 1, 2, 8, 9, 10 (122, 123, 153, 154) Falcipain-2 (155)

Extracellular matrix

Hyaluronidase (156, 157) on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre Iduronate sulfatase (157) -glucuronidase (157)

Membrane channels and signaling Non-junctional connexin 43 hemichannels (89) Na+,K+-ATPase (124) Cystic fibrosis transmembrane regulator (158) Ryanodine receptor 1 (138) GABAA receptors (127, 128) P2X Purinergic receptors (94) P2Y Purinergic receptors (94) N-methyl-D-aspartate receptor (159) DNA-dependent protein kinase (113) Protein kinase C (114) Protein tyrosine phosphatases (117) VIP receptor (129) Follicle-stimulating hormone receptor (131) Pregnane X receptor (137) Diadenosine tetraphosphate hydrolase (160)

Other Prion (PrpC) (136) Complement factors (121, 133–135)

Phospholipase A2 (116, 161) Lysozyme (118) Antimicrobial Peptide CM15 (162) Ubiquitin carboxyl-terminal hydrolases 1 & 2 504865; 463106* HSP 60 chaperonin system (163, 164) GroEL chaperonin system (163, 164) 848 *PubChem BioAssay, last retrieved 29.04.2019

849

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850 Table 4. Solved structures of suramin complexed to target proteins. http://aac.asm.org/ 851

PDB id Protein Reference

6CE2 Myotoxin I from Bothrops moojeni (75) 4YV5 Myotoxin II from Bothrops moojeni (74) 1Y4L Myotoxin II from Bothrops asper (116) on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre 3BJW Ecarpholin S from Echis carinatus (76) 1RML Acid fibroblast growth factor (185) n.a. Human epidermal growth factor (hEGF) (186) 4X3U CBX7 chromodomain (109) 3BF6, 2H9T Human thrombin (187) 2NYR Human sirtuin homolog 5 (112) 3PP7 Leishmania mexicana pyruvate kinase (101) 3GAN Arabidopsis thaliana At3g22680 n.a. 3UR0 Murine norovirus RNA-dependent RNA polymerase (105) 4J4V Pentameric bunyavirus nucleocapsid protein (188) 4J4R Hexameric bunyavirus nucleocapsid protein (188) 852

853

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854 FIGURE LEGENDS http://aac.asm.org/ 855

856 Figure 1. Suramin structure and medicinal chemistry parameters. Except for its good solubility in

857 water, suramin lacks lead-like properties as defined e.g. by Lipinsky's rule of 5.

858

859 Figure 2. Publications on suramin in PubMed. Cumulative numbers are shown for papers on on March 20, 2020 at Brought to you by the University of Dundee Library & Learning Centre

860 suramin and trypanosomes or trypanosomiasis (black, search term "trypanosom*"), cancer (red,

861 "cancer OR tumor"), viruses (yellow, "virus OR viral OR hiv OR aids"), and toxins (green, "toxin

862 OR venom"). Other papers on suramin are shown in beige. There is no saturation yet. And it is

863 surprising that only a minority of the publications on suramin actually deal with trypanosomes.

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